Significant Stability Improvement of Fullerene Organic Photovoltaics via ZnO Film Modification through the Intermittent Spray Pyrolysis Technique

[Image: see text] Morphological control of the layers within the bulk heterojunction organic photovoltaics (BHJ-OPVs) is a key feature that governs their performance. In the present work, we demonstrate that zinc oxide—ZnO—interlayers sprayed via the intermittent spray pyrolysis technique, employing a low-concentration precursor solution, can yield inverted BHJ-OPVs as efficient as the standard reported ones using the conventional laboratory-scale spin-coating technique. However, we record a pioneer stability behavior of the fabricated inverted fullerene organic photovoltaics (iF-OPVs) with various sprayed ZnO conditions. Thus, after optimizing the sprayed ZnO interfacial layer morphology for the inverted PTB7-Th:PC(70)BM devices, by carefully inspecting the interdependence between the sprayed ZnO thin film morphology and the figures of merit of the optimized iF-OPVs, we conducted a distinct analysis on the optical and electronic properties of the fresh and degraded devices using external quantum efficiency measurements and impedance spectroscopy. Hence, we showed that the most proper ZnO microstructural morphology was obtained by spraying 25 running cycles (25R). Remarkably, we observed that 25R-ZnO-based iF-OPV devices showed a stunning stability behavior and maintained 85% of their initial power conversion efficiency even after 16.7 months without encapsulation in a dry nitrogen glovebox, demonstrating an excellent shelf stability. Accordingly, this approach might facilitate the scalability of inverted OPVs for industrial production visibility.